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Transient vibration and product formation of photoexcited CS2 measured by time-resolved X-ray scattering

Transient vibration and product formation of photoexcited CS2 measured by time-resolved X-ray scattering
Transient vibration and product formation of photoexcited CS2 measured by time-resolved X-ray scattering
We have observed details of the internal motion and dissociation channels in photoexcited carbon disulfide (CS2) using time-resolved x-ray scattering (TRXS). Photoexcitation of gas-phase CS2 with a 200 nm laser pulse launches oscillatory bending and stretching motion, leading to dissociation of atomic sulfur in under a picosecond. During the first 300 fs following excitation, we observe significant changes in the vibrational frequency as well as some dissociation of the C–S bond, leading to atomic sulfur in the both 1D and 3P states. Beyond 1400 fs, the dissociation is consistent with primarily 3P atomic sulfur dissociation. This channel-resolved measurement of the dissociation time is based on our analysis of the time-windowed dissociation radial velocity distribution, which is measured using the temporal Fourier transform of the TRXS data aided by a Hough transform that extracts the slopes of linear features in an image. The relative strength of the two dissociation channels reflects both their branching ratio and differences in the spread of their dissociation times. Measuring the time-resolved dissociation radial velocity distribution aids the resolution of discrepancies between models for dissociation proposed by prior photoelectron spectroscopy work.
0021-9606
Gabalski, Ian
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Sere, Malick
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Acheson, Kyle
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Allum, Felix
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Boutet, Sebastien
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Dixit, Gopal
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Forbes, Ruaridh
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Glownia, James M.
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Goff, Nathan
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Hegazy, Kareen
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Howard, Andrew J.
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Liang, Mengning
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Minitti, Michael P.
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Minns, Russell
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Peard, Nolan
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Razmus, Weronika Olimpia
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Sension, Roseanne J
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Ware, Matthew R.
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Weber, Peter M.
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Werby, Nicholas
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Wolf, Thomas J.A.
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Kirrander, Adam
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Bucksbaum, Phillip H.
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Gabalski, Ian
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Sere, Malick
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Acheson, Kyle
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Allum, Felix
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Boutet, Sebastien
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Dixit, Gopal
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Forbes, Ruaridh
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Glownia, James M.
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Goff, Nathan
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Hegazy, Kareen
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Howard, Andrew J.
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Liang, Mengning
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Minitti, Michael P.
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Minns, Russell
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Natan, Adi
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Peard, Nolan
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Razmus, Weronika Olimpia
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Sension, Roseanne J
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Ware, Matthew R.
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Weber, Peter M.
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Werby, Nicholas
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Wolf, Thomas J.A.
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Kirrander, Adam
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Bucksbaum, Phillip H.
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Gabalski, Ian, Sere, Malick, Acheson, Kyle, Allum, Felix, Boutet, Sebastien, Dixit, Gopal, Forbes, Ruaridh, Glownia, James M., Goff, Nathan, Hegazy, Kareen, Howard, Andrew J., Liang, Mengning, Minitti, Michael P., Minns, Russell, Natan, Adi, Peard, Nolan, Razmus, Weronika Olimpia, Sension, Roseanne J, Ware, Matthew R., Weber, Peter M., Werby, Nicholas, Wolf, Thomas J.A., Kirrander, Adam and Bucksbaum, Phillip H. (2022) Transient vibration and product formation of photoexcited CS2 measured by time-resolved X-ray scattering. The Journal of Chemical Physics, 157 (16), [164305]. (doi:10.1063/5.0113079).

Record type: Article

Abstract

We have observed details of the internal motion and dissociation channels in photoexcited carbon disulfide (CS2) using time-resolved x-ray scattering (TRXS). Photoexcitation of gas-phase CS2 with a 200 nm laser pulse launches oscillatory bending and stretching motion, leading to dissociation of atomic sulfur in under a picosecond. During the first 300 fs following excitation, we observe significant changes in the vibrational frequency as well as some dissociation of the C–S bond, leading to atomic sulfur in the both 1D and 3P states. Beyond 1400 fs, the dissociation is consistent with primarily 3P atomic sulfur dissociation. This channel-resolved measurement of the dissociation time is based on our analysis of the time-windowed dissociation radial velocity distribution, which is measured using the temporal Fourier transform of the TRXS data aided by a Hough transform that extracts the slopes of linear features in an image. The relative strength of the two dissociation channels reflects both their branching ratio and differences in the spread of their dissociation times. Measuring the time-resolved dissociation radial velocity distribution aids the resolution of discrepancies between models for dissociation proposed by prior photoelectron spectroscopy work.

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Accepted/In Press date: 3 October 2022
e-pub ahead of print date: 4 October 2022
Published date: 31 October 2022
Additional Information: Funding Information: This work was supported by the AMOS program in the Chemical Sciences, Geosciences, and Biosciences Division of Basic Energy Sciences at the U.S. Department of Energy. I.G. was supported by an NDSEG fellowship. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-76SF00515. This work was also supported by the National Institutes of Health grant, S10 OD025079, via the use of the x-ray detector. W.O.R. acknowledges the STFC XFEL Physical Sciences Hub and the University of Southampton for a Ph.D. studentship. R.S.M. acknowledges financial support from the Leverhulme Trust via Grant No. RPG-2021-257. P.M.W. acknowledges funding by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Award No. DE-SC0017995, and the National Science Foundation, Award No. CHE-1953839. A.K. acknowledges funding from the Engineering and Physical Sciences Research Council (EPSRC), UK, via Grant Nos. EP/V006819 and EP/V049240 and the Leverhulme Trust via Grant No. RPG-2020-208. He also acknowledges a Natural Sciences Fellowship at the Swedish Collegium for Advanced Studies supported by the Erling-Persson Family Foundation and the Knut and Alice Wallenberg Foundation. This work was also supported by the Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DE-SC0020276. K.A. acknowledges an EPSRC Doctoral Studentship from the University of Edinburgh. Publisher Copyright: © 2022 Author(s).
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Identifiers

Local EPrints ID: 471268
URI: http://eprints.soton.ac.uk/id/eprint/471268
DOI: doi:10.1063/5.0113079
ISSN: 0021-9606
PURE UUID: 8905817f-eeb2-4e35-8c82-1cd44ebf9348
ORCID for Russell Minns: ORCID iD orcid.org/0000-0001-6775-2977

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Date deposited: 01 Nov 2022 17:51
Last modified: 17 Mar 2024 03:26

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Contributors

Author: Ian Gabalski
Author: Malick Sere
Author: Kyle Acheson
Author: Felix Allum
Author: Sebastien Boutet
Author: Gopal Dixit
Author: Ruaridh Forbes
Author: James M. Glownia
Author: Nathan Goff
Author: Kareen Hegazy
Author: Andrew J. Howard
Author: Mengning Liang
Author: Michael P. Minitti
Author: Russell Minns ORCID iD
Author: Adi Natan
Author: Nolan Peard
Author: Weronika Olimpia Razmus
Author: Roseanne J Sension
Author: Matthew R. Ware
Author: Peter M. Weber
Author: Nicholas Werby
Author: Thomas J.A. Wolf
Author: Adam Kirrander
Author: Phillip H. Bucksbaum

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